Zinc-ion hybrid capacitors (ZHC) combining many advantages of supercapacitors and batteries, are promising new type of energy storage devices. However, the bottleneck of low energy density and inferior cyclic stability...

Biomass-derived carbons have drawn much attention as electrode materials of supercapacitor due to their low cost, renewability and readily availability. The inherent structure of different biomass greatly affects the microstructure...

Exploration for new layered-structured materials is of significance in multiple fields, e.g., catalysis, energy storage, and conversion, etc. In this work, we develop a visible-light-responsive Sillén-structured mixed-cationic layered catalyst CdBiO2Br based on the typical Sillén-structured BiOBr, and first propose layer structure design as a novel tactic for promoting charge separation and oxygen activation reactions. Differing from BiOBr characterized by [Bi2O2]2+ layer and interleaved Br– double slabs, the crystal structure of CdBiO2Br comprises the [CdBiO2]+ layer and interbedded single Br– slice, rendering a narrowed interlayer spacing from 8.11 to 6.23 Å. The largely reduced interlayer distance drastically shortens the diffusion paths of photogenerated electrons (e – ) and holes (h + ) in CdBiO2Br, allowing favorable migration of carriers from bulk to the surface of the catalysts. Profiting from this structural advantage, CdBiO2Br presents a superior visible-light driven oxygen activation ability in evolution of superoxide radicals (•O2 –) and hydroxyl radicals (•OH), with a production rate of ∼2.4 and 14.1 times that of BiOBr, respectively. DFT calculations unearth that CdBiO2Br has smaller effective masses for both e – and h + than BiOBr, and meanwhile bears a significant difference in the respective mobility of e– and h + , indicative of efficient mobility and separation of carrier charge. In particular, the h + effective mass of CdBiO2Br is merely one-third of that in BiOBr, corresponding well to the far higher •OH generation rate of CdBiO2Br. Our work not only exposes a visible-light-active layered material for environmental chemistry/biochemistry applications but also discloses the huge potential of crystal structure manipulation in governing the charge transport behavior and photo­(electro)­chemical properties.